Millisecond spin coherence of electrons in semiconducting perovskites revealed by spin mode locking

Long spin coherence times of carriers are essential for implementing quantum technologies using semiconductor devices for which, however, a possible obstacle is spin relaxation. For the spin dynamics, decisive features are the band structure, crystal symmetry, and quantum confinement. Perovskite semiconductors recently have come into focus of studies of their spin states, notivated by efficient optical access and potentially long-living coherence. Here, we report an electron spin coherence time T₂ of the order of 1 ms, measured for a bulk FA_0.95Cs_0.05PbI₃ lead halide perovskite crystal. Using periodic laser pulses, we synchronize the electron spin Larmor precession about an external magnetic field in an inhomogeneous ensemble, the effect known as spin mode locking. It appears as a decay of the optically created ensemble spin polarization within the dephasing time T₂^* of up to 20 ns and its revival during the spin coherence time T₂ reaching the millisecond range. This exceptionally long spin coherence time in a bulk crystal is complemented by millisecond-long longitudinal spin relaxation times T₁ for electrons and holes, measured by optically-detected magnetic resonance. These long-lasting spin dynamics highlight perovskites as promising platform for the quantum devices with all-optical control.